Abstract:RuO2 is one of the most important electrocatalyst materials
as a key component of dimensionally stable anode (DSA) for chlorine
evolution reaction, because of the high catalytic activity, while
anodic corrosion remains a fundamental challenge that must be addressed.
Here, we demonstrate that low-temperature annealing of RuO2 nanoparticles (∼1.7 nm) supported on Nb-doped TiO2 leads to the formation of durable active sites with superior activity
and product selectivity toward active chlorine generation (10 mA cm… Show more
“…Other uses for Nb-doped TiO 2 include photovoltaics and dye-sensitized solar cells. − It also finds application in photocatalysis including for the production of H 2 , photoelectrochemical water splitting, and photocatalytic CO 2 reduction . Other catalytic applications are for catalyst supports, for example, for the oxygen reduction reaction and H 2 production, or for dimensionally stable anodes for the chlorine evolution reaction, and electrochemical destruction of “forever chemicals” . Nb-doped TiO 2 has potential application in batteries and supercapacitors including lithium-ion batteries , and Na-ion batteries .…”
Niobium doping of TiO
2
creates a conductive
material
with many new energy applications. When TiO
2
is precipitated
from HCl solutions containing minor Nb, the Nb in solution is quantitatively
deposited with the TiO
2
. Here, we investigate the structure
of Nb doped in anatase and rutile produced from ilmenite digested
in hydrochloric acid. Nb K-edge X-ray absorption near edge structure
(XANES) and extended X-ray absorption fine structure (EXAFS) are used
to characterize the environment of 0.08 atom % Nb doped in TiO
2
. XANES shows clear structural differences between Nb-doped
anatase and rutile. EXAFS for Nb demonstrates that Nb occupies a Ti
site in TiO
2
with no near neighbors of Nb. Hydrolysis of
Ti and Nb from acid solution, followed by calcination, leads to a
well dispersed doped material, with no segregation of Nb. Production
of Nb-doped TiO
2
by this method may be able to supply future
demand for large quantities of the material and in energy applications
where a low cost of production, from readily available natural resources,
would be highly desirable.
“…Other uses for Nb-doped TiO 2 include photovoltaics and dye-sensitized solar cells. − It also finds application in photocatalysis including for the production of H 2 , photoelectrochemical water splitting, and photocatalytic CO 2 reduction . Other catalytic applications are for catalyst supports, for example, for the oxygen reduction reaction and H 2 production, or for dimensionally stable anodes for the chlorine evolution reaction, and electrochemical destruction of “forever chemicals” . Nb-doped TiO 2 has potential application in batteries and supercapacitors including lithium-ion batteries , and Na-ion batteries .…”
Niobium doping of TiO
2
creates a conductive
material
with many new energy applications. When TiO
2
is precipitated
from HCl solutions containing minor Nb, the Nb in solution is quantitatively
deposited with the TiO
2
. Here, we investigate the structure
of Nb doped in anatase and rutile produced from ilmenite digested
in hydrochloric acid. Nb K-edge X-ray absorption near edge structure
(XANES) and extended X-ray absorption fine structure (EXAFS) are used
to characterize the environment of 0.08 atom % Nb doped in TiO
2
. XANES shows clear structural differences between Nb-doped
anatase and rutile. EXAFS for Nb demonstrates that Nb occupies a Ti
site in TiO
2
with no near neighbors of Nb. Hydrolysis of
Ti and Nb from acid solution, followed by calcination, leads to a
well dispersed doped material, with no segregation of Nb. Production
of Nb-doped TiO
2
by this method may be able to supply future
demand for large quantities of the material and in energy applications
where a low cost of production, from readily available natural resources,
would be highly desirable.
“…The crystal structure of the active coating was investigated by XRD (Figure e). Compared with Ti substrate, the additional diffraction peaks of the Ti/RuO 2 porous electrode are attributed to rutile RuO 2 and TiO 2 . The detailed structural information on the coating was further investigated by TEM and SEAD.…”
Section: Resultsmentioning
confidence: 99%
“…Compared with Ti substrate, the additional diffraction peaks of the Ti/RuO 2 porous electrode are attributed to rutile RuO 2 and TiO 2 . 32 The detailed structural information on the coating was further investigated by TEM and SEAD. The lattices with different structural orientations obtained from the TEM image were assigned to TiO 2 (110) and RuO 2 (101) planes (Figure 3f), and the SAED pattern also revealed that the diffraction spots corresponding to the TiO 2 (110) and RuO 2 (101) planes were clearly visible (SI Figure S12).…”
Active chlorine species-mediated
electrocatalytic oxidation is
a promising strategy for ammonia removal in decentralized wastewater
treatment. Flow-through electrodes (FTEs) provide an ideal platform
for this strategy because of enhanced mass transport and sufficient
electrochemically accessible sites. However, limited insight into
spatial distribution of electrochemically accessible sites within
FTEs inhibits the improvement of reactor efficiency and the reduction
of FTE costs. Herein, a microfluidic-based electrochemical system
is developed for the operando observation of microspatial
reactions within pore channels, which reveals that reactions occur
only in the surface layer of the electrode thickness. To further quantify
the spatial distribution, finite element simulations demonstrate that
over 75.0% of the current is accumulated in the 20.0% thickness of
the electrode surface. Based on these findings, a gradient-coated
method for the active layer was proposed and applied to a Ti/RuO2 porous electrode with an optimized pore diameter of ∼25
μm, whose electrochemically accessible surface area was 381.7
times that of the planar electrode while alleviating bubble entrapment.
The optimized reactor enables complete ammonia removal with an energy
consumption of 60.4 kWh kg–1 N, which was 24.2%
and 39.9% less than those with pore diameters of ∼3 μm
and ∼90 μm, respectively.
“…By precisely regulating the fabrication parameters (Table S1), we constructed three kinds of nanostructure-decorated electrodes, including a slab with a large curvature radius of ∼200 nm, nanorods with a curvature radius of ∼25 nm, and nanoneedles with a small curvature radius of ∼10 nm (Figure a–c). As presented by the X-ray diffraction (XRD) pattern, some additional diffraction peaks of the electrodes were assigned to rutile TiO 2 and RuO 2 (Figure d) …”
Section: Results
and Discussionmentioning
confidence: 99%
“…As presented by the X-ray diffraction (XRD) pattern, some additional diffraction peaks of the electrodes were assigned to rutile TiO 2 and RuO 2 (Figure 1d). 17 EDX exhibited a homogeneous distribution of Ti, O, and Ru on the surfaces of the electrodes (Figure 1e). Because the thickness of magnetron-sputtered Ru was only 20 nm, the EDX mapping signal of Ru was visibly weaker than that of Ti, with a Ru content of ∼0.2 g m −2 in the three electrodes.…”
Electrocatalysis applied in energy conversions has recently been associated with nanotips that catalyze extensive fuelforming or value-adding reactions. However, the enhanced catalytic behavior governed by tip-intensified microenvironment reconstruction is particularly elusive and is yet to be understood. Here, we demonstrated a homemade visualization platform to collect information from the local microenvironment of a solution near an electrode (LMSE) with high temporal−spatial resolution, thereby figuring out the sharp-tip enhancement effect for the chlorine evolution reaction (CER). Through visualization using sensitive Cl − and pH sensors, we confirmed that periodic nanoneedles were beneficial for field-induced anion concentration, giving priority to water dissociation and synchronously creating optimal pH conditions for triggering the CER, whereby the Cl − consumption rate within the LMSE was 1.3 times higher than that of the slab counterpart. Tip-enhanced effects meanwhile endowed the local microenvironment with intensified concentration and temperature gradients for continuous transport of Cl − substrates and effective diffusion of HClO products, whereby the oxygen evolution reaction for persistent CER activities was restrained. Our study provides definitive evidence that the optimal microenvironment functionalized with tip-intensified ion concentration from the electrolyte and water dissociation at tip sites are key to stabilize the crucial reaction intermediate for superior electrocatalytic performance.
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